In this paper, the atomic layer deposition (ALD) of ultra-thin films (<4 nm) of Al2O3 and HfO2 on gold-supported monolayer (1L) MoS2 is investigated, providing an insight on the mechanisms ruling the nucleation in the early stages of the ALD process. A preliminary multiscale characterization of large area 1L-MoS2 exfoliated on sputter-grown Au/Ni films demonstrated: (i) a tensile strain (from 0.1 to 0.3%) and p-type doping (from 1 × 1012 to 4 × 1012 cm−2) distribution at micro-scale; (ii) an almost conformal MoS2 membrane to the Au grains topography, with some locally detached regions, indicating the occurrence of strain variations at the nanoscale; (iii) atomic scale variability (from ∼ 4.0 to ∼ 4.5 Å) in the Mo-Au atomic distances was detected, depending on the local configuration of Au nanograins. Ab initio DFT calculations of a free-standing MoS2 layer and a simplified MoS2/Au(1 1 1) interface model showed a …